Plasmonic nanoantennas are versatile tools for coherently controlling and directing light on the nanoscale. For these antennas, current fabrication techniques such as electron beam lithography (EBL) or focused ion beam (FIB) milling with Ga(+)-ions routinely achieve feature sizes in the 10 nm range. However, they suffer increasingly from inherent limitations when a precision of single nanometers down to atomic length scales is required, where exciting quantum mechanical effects are expected to affect the nanoantenna optics. Here, we demonstrate that a combined approach of Ga(+)-FIB and milling-based He(+)-ion lithography (HIL) for the fabrication of nanoantennas offers to readily overcome some of these limitations. Gold bowtie antennas with 6 nm gap size were fabricated with single-nanometer accuracy and high reproducibility. Using third harmonic (TH) spectroscopy, we find a substantial enhancement of the nonlinear emission intensity of single HIL-antennas compared to those produced by state-of-the-art gallium-based milling. Moreover, HIL-antennas show a vastly improved polarization contrast. This superior nonlinear performance of HIL-derived plasmonic structures is an excellent testimonial to the application of He(+)-ion beam milling for ultrahigh precision nanofabrication, which in turn can be viewed as a stepping stone to mastering quantum optical investigations in the near-field.
Structural
diffraction analysis of an anilino squaraine with branched isobutyl side chains shows crystallization into
two polymorphic structures in the bulk and in spin-casted thin films.
We observe multipeaked and pleochroic absorption spectra being blue-(red)-shifted
for the monoclinic (orthorhombic) polymorph. We understand the packing
as Coulombic molecular H-(J)-aggregates supporting Davydov splitting.
Pictures of projected Davydov components in oriented thin films fit
well to polarization resolved spectro-microscopy and crossed-polarized
light microscopy investigations. By comparison with literature on
anilino squaraines with linear alkyl side chains,
we point out a general trend for steering the thin film excitonic
properties by simple side chain and/or processing condition variation.
Combined with the ability to locally probe the direction of transition
dipole moments, this adds value to the rational design of functional
thin films for optoelectronic applications, especially envisioning
ultrastrong light–matter interactions.
Chiral plasmonic nanostructures will be of increasing importance for future applications in the field of nano optics and metamaterials. Their sensitivity to incident circularly polarized light in combination with the ability of extreme electromagnetic field localization renders them ideal candidates for chiral sensing and for all-optical information processing. Here, the resonant modes of single plasmonic helices are investigated. We find that a single plasmonic helix can be efficiently excited with circularly polarized light of both equal and opposite handedness relative to that of the helix. An analytic model provides resonance conditions matching the results of full-field modeling. The underlying geometric considerations explain the mechanism of excitation and deliver quantitative design rules for plasmonic helices being resonant in a desired wavelength range. Based on the developed analytical design tool, single silver helices were fabricated and optically characterized. They show the expected strong chiroptical response to both handednesses in the targeted visible range. With a value of 0.45 the experimentally realized dissymmetry factor is the largest obtained for single plasmonic helices in the visible range up to now. arXiv:1811.04851v2 [physics.optics]
The nonlinear optical properties of thin ZnO film are studied using interferometric autocorrelation (IFRAC) microscopy. Ultrafast, below-bandgap excitation with 6-fs laser pulses at 800 nm focused to a spot size of 1 µm results in two emission bands in the blue and blue-green spectral region with distinctly different coherence properties. We show that an analysis of the wavelength-dependence of the interference fringes in the IFRAC signal allows for an unambiguous assignment of these bands as coherent second harmonic emission and incoherent, multiphoton-induced photoluminescence, respectively. More generally our analysis shows that IFRAC allows for a complete characterization of the coherence properties of the nonlinear optical emission from nanostructures in a single-beam experiment. Since this technique combines a very high temporal and spatial resolution we anticipate broad applications in nonlinear nano-optics.
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